JP5958889B2 - Method for immobilizing carbon in carbon dioxide - Google Patents
Method for immobilizing carbon in carbon dioxide Download PDFInfo
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- JP5958889B2 JP5958889B2 JP2008003187A JP2008003187A JP5958889B2 JP 5958889 B2 JP5958889 B2 JP 5958889B2 JP 2008003187 A JP2008003187 A JP 2008003187A JP 2008003187 A JP2008003187 A JP 2008003187A JP 5958889 B2 JP5958889 B2 JP 5958889B2
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims description 174
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims description 87
- 239000001569 carbon dioxide Substances 0.000 title claims description 85
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims description 20
- 229910052799 carbon Inorganic materials 0.000 title claims description 20
- 238000000034 method Methods 0.000 title description 10
- 230000003100 immobilizing effect Effects 0.000 title description 4
- 239000011575 calcium Substances 0.000 claims description 48
- 229910052791 calcium Inorganic materials 0.000 claims description 36
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 35
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims description 30
- 239000000292 calcium oxide Substances 0.000 claims description 28
- 239000007788 liquid Substances 0.000 claims description 28
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims description 27
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims description 17
- 239000000920 calcium hydroxide Substances 0.000 claims description 16
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims description 16
- 238000002347 injection Methods 0.000 claims description 9
- 239000007924 injection Substances 0.000 claims description 9
- 239000007787 solid Substances 0.000 claims description 6
- 238000006243 chemical reaction Methods 0.000 claims description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- 230000003116 impacting effect Effects 0.000 claims description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 24
- 239000007789 gas Substances 0.000 description 19
- 150000001875 compounds Chemical class 0.000 description 11
- 239000000126 substance Substances 0.000 description 10
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 9
- 239000007921 spray Substances 0.000 description 9
- 229910021532 Calcite Inorganic materials 0.000 description 8
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 8
- 238000010521 absorption reaction Methods 0.000 description 6
- 229940043430 calcium compound Drugs 0.000 description 5
- 150000001674 calcium compounds Chemical class 0.000 description 5
- 239000000203 mixture Substances 0.000 description 5
- 239000000243 solution Substances 0.000 description 5
- 229910000019 calcium carbonate Inorganic materials 0.000 description 4
- 230000007423 decrease Effects 0.000 description 4
- 239000010419 fine particle Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 150000001350 alkyl halides Chemical class 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 238000011084 recovery Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 239000002244 precipitate Substances 0.000 description 2
- 238000005507 spraying Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 238000010998 test method Methods 0.000 description 2
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 description 1
- 235000019738 Limestone Nutrition 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- 229910052772 Samarium Inorganic materials 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- -1 calcium metal Chemical class 0.000 description 1
- JYYOBHFYCIDXHH-UHFFFAOYSA-N carbonic acid;hydrate Chemical compound O.OC(O)=O JYYOBHFYCIDXHH-UHFFFAOYSA-N 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000004567 concrete Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical compound [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 239000011630 iodine Substances 0.000 description 1
- 229910052740 iodine Inorganic materials 0.000 description 1
- 239000006028 limestone Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000004579 marble Substances 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
- WJCNZQLZVWNLKY-UHFFFAOYSA-N thiabendazole Chemical compound S1C=NC(C=2NC3=CC=CC=C3N=2)=C1 WJCNZQLZVWNLKY-UHFFFAOYSA-N 0.000 description 1
- XQKBFQXWZCFNFF-UHFFFAOYSA-K triiodosamarium Chemical compound I[Sm](I)I XQKBFQXWZCFNFF-UHFFFAOYSA-K 0.000 description 1
- 239000011882 ultra-fine particle Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
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- Gas Separation By Absorption (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Compounds Of Alkaline-Earth Elements, Aluminum Or Rare-Earth Metals (AREA)
- Carbon And Carbon Compounds (AREA)
Description
本発明は、カルシウム又はカルシウム化合物に衝撃を与えることにより二酸化炭素（ＣＯ２）中の炭素を固定する方法に関する。 The present invention relates to a method for fixing carbon in carbon dioxide (CO 2 ) by impacting calcium or calcium compounds.
化石燃料の燃焼によって発生する二酸化炭素が温室効果による地球温暖化の原因物質であることから、二酸化炭素を固定化するための技術の開発が進められている。 Since carbon dioxide generated by the combustion of fossil fuel is a causative substance of global warming due to the greenhouse effect, development of a technology for fixing carbon dioxide is being promoted.
二酸化炭素を固定化する最も簡単な方法は、二酸化炭素を含むガスをアルカリ性水溶液と接触させて、炭酸塩として除去する方法が考えられる。 The simplest method for immobilizing carbon dioxide is a method in which a gas containing carbon dioxide is brought into contact with an alkaline aqueous solution and removed as a carbonate.
しかし、この方法では、回収された炭酸塩が稀薄な溶液であったり、或いは不純物等も夾雑したりして、何ら利用することができない。また、アルカリ源として水酸化カルシウムを用いれば、炭酸カルシウムの沈殿として回収は可能であるが、水酸化カルシウムの溶解度が小さいため、大量の溶液が必要であるとか、沈殿物が装置に詰まるなど、効率よく二酸化炭素を固定化することができない。 However, this method cannot be used at all because the recovered carbonate is a dilute solution or impurities are contaminated. In addition, if calcium hydroxide is used as the alkali source, it can be recovered as calcium carbonate precipitate, but since the solubility of calcium hydroxide is small, a large amount of solution is required, or the precipitate is clogged in the device, etc. Carbon dioxide cannot be immobilized efficiently.
そこで、特許文献１には、効率よく二酸化炭素を固定することができる二酸化炭素固定溶液として、サマリウムと、ヨウ化サマリウムと、ハロゲン化アルキル（３）を使用し、この二酸化炭素固定溶液に光を照射することによって、上記二酸化炭素固定溶液に溶解した二酸化炭素とハロゲン化アルキル（３）とを反応させて二酸化炭素を固定する二酸化炭素固定方法が開示されている。 Therefore, in Patent Document 1, samarium, samarium iodide, and alkyl halide (3) are used as a carbon dioxide fixing solution capable of efficiently fixing carbon dioxide, and light is supplied to the carbon dioxide fixing solution. A carbon dioxide fixing method is disclosed in which carbon dioxide dissolved in the carbon dioxide fixing solution is reacted with an alkyl halide (3) to fix the carbon dioxide.
また、特許文献２には、二酸化炭素を有用な物質の生成に利用して固定することができる二酸化炭素固定方法として、吸収塔から排出される吸収液を、貯留槽を介して吸収塔に還流させ、排ガスと吸収液とを気液接触させて、吸収液の水素イオン指数が所定の値となった場合に、吸収液にアルカリ水を混入して炭酸塩水を生成する。そして、炭酸塩水に水酸化カルシウム水を混入し、炭酸カルシウムを析出させ、二酸化炭素を有用な炭酸カルシウムの生成に利用して固定することが開示されている。 Further, in Patent Document 2, as a carbon dioxide fixing method capable of fixing carbon dioxide using a useful substance, the absorption liquid discharged from the absorption tower is returned to the absorption tower via a storage tank. When the exhaust gas and the absorption liquid are brought into gas-liquid contact, and the hydrogen ion index of the absorption liquid reaches a predetermined value, alkaline water is mixed into the absorption liquid to generate carbonate water. And it is disclosed that calcium hydroxide water is mixed in carbonated water to precipitate calcium carbonate, and carbon dioxide is used and fixed for producing useful calcium carbonate.
これらの方法は、二酸化炭素を有効利用することは可能ではあるが、回収コストが高くなり、実用性に難がある。
本発明は、安価で容易に入手できるカルシウム又はカルシウム化合物を用いて簡単な操作により二酸化炭素中の炭素を固定する方法を提供するものである。 The present invention provides a method for fixing carbon in carbon dioxide by a simple operation using calcium or a calcium compound that is inexpensive and easily available.
すなわち、本願請求項１に係る発明は、二酸化炭素を溶解する液体媒体中に固体であるカルシウム、酸化カルシウム又は水酸化カルシウムを入れ、該液体媒体中に二酸化炭素を０．２ＭＰａ以上の噴射圧で直接噴射して該液体媒体中に二酸化炭素を供給し、存在させると共に、併せて該液体媒体を動揺させることにより、前記液体媒体を介して前記カルシウム、酸化カルシウム又は水酸化カルシウムに衝撃を与えながら前記カルシウム、酸化カルシウム又は水酸化カルシウムと二酸化炭素とを接触させるとともに、前記カルシウム、酸化カルシウム又は水酸化カルシウムは前記二酸化炭素を直接噴射する段階において固体のまま液体媒体中に存在させて化学反応を行わせることにより前記カルシウム、酸化カルシウム又は水酸化カルシウムが炭素及び酸素と化学量論的な結合及び不定比状態で結合した状態で二酸化炭素中の炭素を固定化する方法である。 That is, in the invention according to claim 1 of the present application, solid calcium, calcium oxide or calcium hydroxide is placed in a liquid medium in which carbon dioxide is dissolved, and carbon dioxide is injected into the liquid medium at an injection pressure of 0.2 MPa or more. While directly injecting and supplying carbon dioxide into the liquid medium and causing the liquid medium to be shaken, while impacting the calcium, calcium oxide or calcium hydroxide through the liquid medium The calcium, calcium oxide, or calcium hydroxide is brought into contact with carbon dioxide, and the calcium, calcium oxide, or calcium hydroxide is allowed to exist in a liquid medium as a solid in the step of directly injecting the carbon dioxide, thereby causing a chemical reaction. By making the calcium, calcium oxide or calcium hydroxide A method for immobilizing the carbon in the carbon dioxide remain attached with iodine and oxygen stoichiometric binding and non-stoichiometric state.
上記請求項１に係る発明において、カルシウム又はカルシウム含有化合物に衝撃を与える手段として好ましい態様は、固体状のカルシウム又はカルシウム含有化合物に直接二酸化炭素を噴射する手段である。この場合の噴射圧は、０．２ＭＰａ以上、好ましくは、０．５ＭＰａであり、１ＭＰａを超えても効果はあまり変わらない。 In the invention according to the first aspect, a preferred aspect as means for giving an impact to calcium or a calcium-containing compound is means for directly injecting carbon dioxide into solid calcium or a calcium-containing compound. The injection pressure in this case is 0.2 MPa or more, preferably 0.5 MPa, and the effect does not change much even if it exceeds 1 MPa.
本発明において、好ましい衝撃付与の手段として、カルシウム又はカルシウム含有化合物を液体媒体中に入れ、該液体媒体中に二酸化炭素を噴射する手段である。この場合、二酸化炭素は液体媒体中に溶解し、カルシウム又はカルシウム含有化合物の周辺に存在することになり、しかも、二酸化炭素を高速で噴射することにより液を動揺させることができる。このため、例えば０．２ＭＰａ以上、好ましくは０．５ＭＰａ程度の高圧で二酸化炭素を液中に噴射するか、或いは別途攪拌器により、液体媒体を高速で攪拌する手段や、ポンプ液体媒体を高速循環させる手段を併用することにより一層の効果を得ることができる。 In the present invention, as a preferable means for imparting impact, calcium or a calcium-containing compound is placed in a liquid medium, and carbon dioxide is injected into the liquid medium. In this case, carbon dioxide is dissolved in the liquid medium and is present around calcium or the calcium-containing compound, and the liquid can be shaken by jetting carbon dioxide at a high speed. For this reason, for example, carbon dioxide is injected into the liquid at a high pressure of 0.2 MPa or more, preferably about 0.5 MPa, or a means for stirring the liquid medium at a high speed by a separate stirrer or a pump liquid medium is circulated at high speed. A further effect can be obtained by using a combination of the above means.
また、液体媒体としては、水が一般的であるが、メタノール、エタノールあるいはイソプロパノール等のアルコール類、更にはベンゼン、トルエン、キシレン等の炭化水素類等、二酸化炭素を比較的溶解しやすい液体媒体も有効に使用することができる。 In addition, water is generally used as the liquid medium, but liquid media that are relatively easy to dissolve carbon dioxide, such as alcohols such as methanol, ethanol, and isopropanol, and hydrocarbons such as benzene, toluene, and xylene, are also available. It can be used effectively.
本発明において、二酸化炭素中の炭素を固定化するとは、カルシウム又はカルシウム含有化合物が炭素及び酸素と化学量論的な結合のみならず、不定比状態で結合した状態をとり、結果として二酸化炭素由来の炭素が固定化されていることを意味するものである。かかる固定化を単に二酸化炭素を固定化するとも言い、得られる化合物を不定比含炭素カルシウム化合物という。 In the present invention, the fixation of carbon in carbon dioxide means that calcium or a calcium-containing compound is not only stoichiometrically bonded to carbon and oxygen, but is also bonded in an unstoichiometric state, resulting in carbon dioxide. This means that the carbon is immobilized. Such immobilization is also simply referred to as immobilizing carbon dioxide, and the resulting compound is referred to as a non-stoichiometric carbon-containing calcium compound.
また、本発明において用いられるカルシウム又はカルシウム含有化合物とは、カルシウム金属及び酸化カルシウム、水酸化カルシウム、カルシウム含有鉱物、例えば方解石、大理石、石灰岩、セメント、コンクリート等、カルシウムを成分として含有する物質であって、中でも、金属カルシウム、酸化カルシウム及び水酸化カルシウムが好適に用いられる。 The calcium or calcium-containing compound used in the present invention is a substance containing calcium as a component, such as calcium metal and calcium oxide, calcium hydroxide, calcium-containing minerals such as calcite, marble, limestone, cement, and concrete. Among these, metallic calcium, calcium oxide, and calcium hydroxide are preferably used.
本発明は、安価で容易に入手できる固体であるカルシウムあるいはカルシウム化合物に二酸化炭素を噴射するだけの簡単な操作で二酸化炭素を固定化することができる。 According to the present invention, carbon dioxide can be fixed by a simple operation of injecting carbon dioxide onto calcium or a calcium compound, which is a cheap and easily available solid.
本発明の最大の特徴は、衝撃を与えながらカルシウム又はカルシウム含有化合物と二酸化炭素とを接触させることにより動的条件下に化学反応を行わせることにある。このため、静的条件下では、化学量論的な反応しか生じない。例えば水酸化カルシウムと二酸化炭素は水の共存下では単に炭酸カルシウム（ＣａＣＯ３）を生成するだけであるが、本発明にあっては単にＣａＣＯ３の生成のみならず、場合によっては炭素の単体からＣａＣｘＯｙ（但し、ｘ、ｙはそれぞれ任意の数）のカルシウム、炭素及び酸素の不定比の化合物よりなる混合物として得られるのである。その一例を図１に示す。 The greatest feature of the present invention is that a chemical reaction is performed under dynamic conditions by bringing calcium or a calcium-containing compound into contact with carbon dioxide while giving an impact. For this reason, only stoichiometric reactions occur under static conditions. For example, calcium hydroxide and carbon dioxide merely produce calcium carbonate (CaCO 3 ) in the presence of water, but in the present invention, not only the production of CaCO 3 , but also from the simple substance of carbon in some cases. It is obtained as a mixture of CaCxOy (where x and y are each an arbitrary number) calcium, carbon and oxygen non-stoichiometric compounds. An example is shown in FIG.
図１は、本発明の実施として炭酸ガス・スプレー（ガス圧、約０．２ＭＰａ）を用い、常温下に金属カルシウムに１０秒間炭酸ガスを噴射した場合の生成物におけるＣａＯとＣＯ２の割合を示す図である。もし生成物がＣａＣＯ３であれば、ＣａＯとＣＯ２との割合はＣａＯ＝５６％、ＣＯ２＝４４％となるはずであるが、図１においてはＣＯ２＝０から６０％まで、それに対してＣａＯは、ＣａＯ＝１００から４０％の化合物が生成している。 FIG. 1 shows the ratio of CaO and CO2 in a product when carbon dioxide spray (gas pressure, about 0.2 MPa) is used as an embodiment of the present invention and carbon dioxide is injected into metallic calcium for 10 seconds at room temperature. FIG. If the product is CaCO 3, the ratio between CaO and CO 2 is CaO = 56%, but should be CO 2 = 44%, up to 60% CO 2 = 0 in FIG. 1, contrast In CaO, CaO = 100 to 40% of a compound is generated.
本発明を実施例により説明する。 The present invention is illustrated by examples.
１．使用薬品
（１） カルシウム（Ｃａ）（キシダ化学（株）製，９９％）
（２）炭酸ガス・スプレー（中村理科工業製，９５％および大陽白酸，９９．９％
２．試験方法
Ｃａをガラスプレートの上に両面テープで留め置き、このＣａに炭酸ガス・スプレーによりＣＯ２を照射した。照射温度は常温（２４℃）および高温（８５℃）で行った。
1. Chemicals used (1) Calcium (Ca) (manufactured by Kishida Chemical Co., Ltd., 99%)
(2) Carbon dioxide spray (Nakamura Rika Kogyo, 95% and Taiyoshiro acid, 99.9%
2. Test method Ca was fixed on a glass plate with double-sided tape, and this Ca was irradiated with CO 2 by a carbon dioxide spray. Irradiation temperature was normal temperature (24 degreeC) and high temperature (85 degreeC).
３．試験結果
（１）常温（２４℃）で１０秒間炭酸ガス・スプレーの照射：ＣＯ２＝７〜１５％がＣａと反応。生成物は炭酸塩質であった。
3. Test result (1) Carbon dioxide spray irradiation at room temperature (24 ° C.) for 10 seconds: CO 2 = 7 to 15% reacts with Ca. The product was carbonated.
（２）高温（８５℃）で１０秒間炭酸ガス・スプレーの照射：ＣＯ２＝１５〜４３％がＣａと反応。方解石はＣＯ２＝４４％なので、高温で方解石組成がわずか生成していた。生成した炭酸塩微粒子は、１μｍサイズの微粒子の集合体であった。 (2) Carbon dioxide spray irradiation at high temperature (85 ° C.) for 10 seconds: CO 2 = 15-43% reacts with Ca. Since calcite is CO 2 = 44%, a slight calcite composition was produced at high temperature. The produced carbonate fine particles were aggregates of fine particles having a size of 1 μm.
１．使用薬品
酸化カルシウム（ＣａＯ）（キシダ化学（株）製，９８％）
２．試験方法
ＣａＯをガラスプレートの上に両面テープで留め置き、このＣａＯに炭酸ガス・スプレーでＣＯ２を照射した。
1. Chemicals used: calcium oxide (CaO) (Kishida Chemical Co., Ltd., 98%)
2. Test Method CaO was fixed on a glass plate with double-sided tape, and this CaO was irradiated with CO2 with a carbon dioxide spray.
照射温度は常温（２４℃）および高温（８５℃）で行った。車の排気ガス（駐車時始発前と３０分走行後８５℃）についても試験した。 Irradiation temperature was normal temperature (24 degreeC) and high temperature (85 degreeC). It was also tested for car exhaust (before parking and at 85 ° C for 30 minutes after parking).
３．試験結果
（１）常温（２４℃）で１０秒間炭酸ガス・スプレーの照射：ＣＯ２＝１１〜２４％がＣａＯと反応。方解石でなく、炭酸塩質であった。
3. Test result (1) Carbon dioxide spray irradiation at room temperature (24 ° C.) for 10 seconds: CO 2 = 11 to 24% reacted with CaO. It was not calcite but carbonate.
（２）高温（８５℃）で１０〜６０秒間照射：ＣＯ２＝２２−５９％がＣａＯと反応。 (2) Irradiation at high temperature (85 ° C.) for 10-60 seconds: CO 2 = 22-59% reacts with CaO.
（３）車の始発時の低温ガス：ＣＯ２＝２２〜２５％、
（４）３０分走行後の８５℃以上の高温ガスによる吹き付け：ＣＯ２＝２９〜５９％の増加。方解石はＣＯ２＝４４％なので、高温で方解石組成がわずか生成していた。生成した炭酸塩微粒子は、１μｍサイズの微粒子の集合体であった。
(3) vehicle initial set time of the cold gas: CO 2 = 22~25%,
(4) Spraying with high-temperature gas at 85 ° C. or higher after running for 30 minutes: CO 2 = 29 to 59% increase. Since calcite is CO 2 = 44%, a slight calcite composition was produced at high temperature. The produced carbonate fine particles were aggregates of fine particles having a size of 1 μm.
１．使用薬品、測定器
（１）カルシウム（Ｃａ）．：キシダ化学（株）製，Ｌｏ．Ｎｏ．Ｍ１７７６５Ｖ，９９％）
（２）酸化カルシウム（ＣａＯ）：キシダ化学（株）製，Ｌｏ．Ｎｏ．Ｅｌ０１４８Ｖ，９８％）
（３）水酸化カルシウム（Ｃａ（ＯＨ）２）：キシダ化学（株）製，Ｌｏ．Ｎｏ．０１０−１３６０５，９５％
（４）炭酸ガス・スプレー（中村理科工業製，９５％，および大陽白酸製，９９．９％）
大気中の炭酸ガス測定器：赤外線ＣＯ２モニター（理研計器，ＲＩ−８５）
マルチ検出器ｔｅｓｔｏ５３５（（株）テストー製）
水中の炭酸ガス測定器：Ｔ−ｉ９００４（（株）東興化学研究所製）
２．実験方法
（１）炭酸ガスから水中に溶ける炭酸ガスの測定
水中に直接炭酸ガスノズルで注入した時間変化量を３回行い、いずれも５秒間炭酸ガス噴射で水中の炭酸ガス量が８２〜１３３（ｍｇ／ｌ）から４１０〜４５７（ｍｇ／ｌ）に増加し、その後１０秒間照射で５５６〜９９４（ｍｇ／１）に急増した。１５秒間噴射で１１０６（ｍｇ／ｌ）の１０倍に増加した（水に炭酸ガスが注入されると溶解する。）。
1. Chemicals used, measuring instrument (1) Calcium (Ca). : Kishida Chemical Co., Ltd., Lo. No. M17765V, 99%)
(2) Calcium oxide (CaO): manufactured by Kishida Chemical Co., Ltd., Lo. No. El0148V, 98%)
(3) Calcium hydroxide (Ca (OH) 2 ): manufactured by Kishida Chemical Co., Ltd., Lo. No. 010-13605, 95%
(4) Carbon dioxide spray (manufactured by Nakamura Rika Kogyo, 95%, and Taiyoshiro acid, 99.9%)
Carbon dioxide gas measuring instrument in the atmosphere: Infrared CO 2 monitor (RIKEN Keiki, RI-85)
Multi detector testo 535 (manufactured by Testo Co., Ltd.)
Underwater carbon dioxide meter: Ti9004 (manufactured by Toko Chemical Laboratory Co., Ltd.)
2. Experimental method (1) Measurement of carbon dioxide dissolved in water from carbon dioxide gas The amount of time change injected directly into the water with a carbon dioxide nozzle was performed three times, and in each case, carbon dioxide gas in water was 82 to 133 (mg) by carbon dioxide gas injection. / L) to 410 to 457 (mg / l), and then rapidly increased to 556 to 994 (mg / 1) by irradiation for 10 seconds. It increased to 10 times 1106 (mg / l) by spraying for 15 seconds (dissolves when carbon dioxide is injected into water).
（２）炭酸ガスが水中から大気中に散逸する炭酸ガスの測定
水中の炭酸ガスは、炭素固定にはならないため、時間と共に減少する。前記の１１０６ｍｇ／１の高い炭酸ガス量が１時間半後に元の炭酸ガス量の３３６ｍｇ／ｌになり、３０％の割合に減少する。
(2) Measurement of carbon dioxide in which carbon dioxide is dissipated from water to the atmosphere Carbon dioxide in water does not become carbon-fixed and therefore decreases with time. The high carbon dioxide gas amount of 1106 mg / 1 becomes 336 mg / l of the original carbon dioxide gas amount after 1 hour and a half, and decreases to a rate of 30%.
回転子で動的に撹拌すると、ある回転数（＞１５００ｒｐｍ）から炭酸ガス量が水中から急減し空気中に散逸する。これは、炭酸ガスが、水中に反応物（Ｃａ含有物など）がないと、空気中に逸散することを示す。実際１２００ｒｐｍで９３０（ｍｇ／ｌ）そして１５５０ｒｐｍで１８００（ｍｇ／ｌ）になる。 When agitating dynamically with a rotor, the amount of carbon dioxide decreases rapidly from the water at a certain rotational speed (> 1500 rpm) and dissipates into the air. This indicates that carbon dioxide escapes into the air if there are no reactants (such as Ca-containing materials) in the water. In fact, it becomes 930 (mg / l) at 1200 rpm and 1800 (mg / l) at 1550 rpm.
水中の炭酸ガス量が減少するため、持続的に炭酸ガスを水中に注入すると、ほぼ維持され、注入がないと炭酸ガスは空中に散逸する。 Since the amount of carbon dioxide in the water decreases, if carbon dioxide is continuously injected into the water, it is almost maintained, and if there is no injection, the carbon dioxide is dissipated into the air.
（３）炭酸ガスを水中に噴射してできたＣａ含有試料（Ｃａ，ＣａＯ，Ｃａ（ＯＨ）２）に吸着される炭酸ガスの測定
ＣａとＣａＯを水中に入れて炭酸ガスを動的注入し撹拌（８００ｒｐｍ）（２５℃）すると、水中の炭酸ガス量が半減する（１分以内の現象）。実際７３（ｍｇ／ｌ）が５〜１５秒間のガス注入で２５（ｍｇ／１）に減少し、これが炭酸塩に炭素固定された量に相当する。
(3) Measurement of carbon dioxide adsorbed on a Ca-containing sample (Ca, CaO, Ca (OH) 2 ) produced by injecting carbon dioxide into water Ca and CaO are placed in water and carbon dioxide is dynamically injected. When stirring (800 rpm) (25 ° C.), the amount of carbon dioxide in water is halved (a phenomenon within 1 minute). In fact, 73 (mg / l) is reduced to 25 (mg / 1) by gas injection for 5 to 15 seconds, which corresponds to the amount of carbon fixed to the carbonate.
Ｃａ（ＯＨ）２を水中に入れて炭酸ガスを動的注入し撹拌（８００ｒｐｍ）（２５℃）しても、水中の炭酸ガス量が不変である。２５（ｍｇ／ｌ）が５〜１５秒間のガス注入で３３（ｍｇ／１）になった。 Even when Ca (OH) 2 is put in water and carbon dioxide is dynamically injected and stirred (800 rpm) (25 ° C.), the amount of carbon dioxide in the water remains unchanged. 25 (mg / l) became 33 (mg / 1) by gas injection for 5 to 15 seconds.
この現象は、長持間（約２４００分）にわたり炭酸ガスの液中注入を繰り返すと、水中の炭酸ガスの急増がなく、継続的にＣａ含有物と反応していることを示す。 This phenomenon indicates that when carbon dioxide gas injection in the liquid is repeated over a long period of time (about 2400 minutes), there is no sudden increase in carbon dioxide gas in the water, and it continuously reacts with the Ca-containing material.
液体中に生成した炭酸塩物質には、ナノ炭酸塩の形成が観察できた。方解石質組成相などの炭酸塩物質の形成により、炭酸ガスから水中で多量の炭素の固定を再現できた。 Nanocarbonate formation could be observed in the carbonate material formed in the liquid. Due to the formation of carbonate materials such as calcite composition phase, a large amount of carbon fixation from carbon dioxide gas in water could be reproduced.
水中で炭素固定した炭酸塩物質（方解石質構造）は、広く分散して極微細粒子（約１００ｎｍ）で生成していることが始めてわかった。板状の粒子には炭素が多い（７０％ＣＯ２）ことが始めてわかった。 It was found for the first time that carbonate substances (calcite structure) fixed with carbon in water were widely dispersed and formed as ultrafine particles (about 100 nm). It was found for the first time that the plate-like particles are rich in carbon (70% CO 2 ).
１．使用薬品
（１） 酸化カルシウム（ＣａＯ，キシダ化学（株）製，Ｌｏ．Ｎｏ．Ｅ１０１４８Ｖ，９８％）
（２） 炭酸ガス・スプレー（中村理科工業，９５％および大陽白酸，９９．９％）
２．実験方法
ＣａＯ約２グラムを秤量し、炭酸ガスを水中で照射し、高温、マグネットによる回転で実験し、ろ紙でろ過して、回収した量を比較した。一般に炭酸ガスと反応すれば、炭素固定が顕著な試料では回収量が多くなると考えられる。
1. Chemicals used (1) Calcium oxide (CaO, manufactured by Kishida Chemical Co., Ltd., Lo. No. E10148V, 98%)
(2) Carbon dioxide spray (Nakamura Science, 95% and Taiyoshiro acid, 99.9%)
2. Experimental Method About 2 grams of CaO was weighed, carbon dioxide was irradiated in water, the experiment was performed at high temperature and rotation with a magnet, filtered through filter paper, and the recovered amounts were compared. In general, if it reacts with carbon dioxide gas, it is considered that the amount recovered is increased in a sample with remarkable carbon fixation.
炭酸ガスの急激な照射で動的反応をさせて、回収量の最大となる条件を求めるために液中に回転子を入れて、２０００回転（ｒｐｍ）まで変化させる。 A dynamic reaction is caused by rapid irradiation of carbon dioxide gas, and a rotor is put in the liquid in order to obtain a condition for maximizing the recovery amount, and the rotation is changed to 2000 rpm.
３．試験結果
９０℃近くに試料全体の重さによる回収量の最大が現れる。その回収量は、約２倍以上に及ぶ。回転１，３００（ｒｐｍ）、炭酸ガス液中照射３０秒間である。
3. Test results The maximum recovery amount due to the weight of the entire sample appears near 90 ° C. The amount collected is about twice or more. The rotation is 1,300 (rpm) and the irradiation is in carbon dioxide gas for 30 seconds.
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